Achieving Ultra-Broad Microwave Absorption Bandwidth Around Millimeter-Wave Atmospheric Window Through an Intentional Manipulation on Multi-Magnetic Resonance Behavior

The utilization of electromagnetic waves is rapidly advancing into the millimeter-wave frequency range, posing increasingly severe challenges in terms of electromagnetic pollution prevention and radar stealth. However, existing millimeter-wave absorbers are still inadequate in addressing these issues due to their monotonous magnetic resonance pattern. In this work, rare-earth La³⁺ and non-magnetic Zr⁴⁺ ions are simultaneously incorporated into M-type barium ferrite (BaM) to intentionally manipulate the multi-magnetic resonance behavior. By leveraging the contrary impact of La³⁺ and Zr⁴⁺ ions on magnetocrystalline anisotropy field, the restrictive relationship between intensity and frequency of the multi-magnetic resonance is successfully eliminated. The magnetic resonance peak-differentiating and imitating results confirm that significant multi-magnetic resonance phenomenon emerges around 35 GHz due to the reinforced exchange coupling effect between Fe³⁺ and Fe²⁺ ions. Additionally, Mössbauer spectra analysis, first-principle calculations, and least square fitting collectively identify that additional La³⁺ doping leads to a profound rearrangement of Zr⁴⁺ occupation and thus makes the portion of polarization/conduction loss increase gradually. As a consequence, the La³⁺–Zr⁴⁺ co-doped BaM achieves an ultra-broad bandwidth of 12.5 + GHz covering from 27.5 to 40 + GHz, which holds remarkable potential for millimeter-wave absorbers around the atmospheric window of 35 GHz.